Buckling of paramagnetic chains in soft gels.

We study the magneto-elastic coupling behavior of paramagnetic chains in soft polymer gels exposed to external magnetic fields. To this end, a laser scanning confocal microscope is used to observe the morphology of the paramagnetic chains together with the deformation field of the surrounding gel network. The paramagnetic chains in soft polymer gels show rich morphological shape changes under oblique magnetic fields, in particular a pronounced buckling deformation. The details of the resulting morphological shapes depend on the length of the chain, the strength of the external magnetic field, and the modulus of the gel. Based on the observation that the magnetic chains are strongly coupled to the surrounding polymer network, a simplified model is developed to describe their buckling behavior. A coarse-grained molecular dynamics simulation model featuring an increased matrix stiffness on the surfaces of the particles leads to morphologies in agreement with the experimentally observed buckling effects.

Superelastic stress-strain behavior in ferrogels with different types of magneto-elastic coupling.

Colloidal magnetic particles embedded in an elastic polymer matrix constitute a smart material called a ferrogel. It responds to an applied external magnetic field by changes in elastic properties, which can be exploited for various applications such as dampers, vibration absorbers, or actuators. Under appropriate conditions, the stress-strain behavior of a ferrogel can display a fascinating feature: superelasticity, the capability to reversibly deform by a huge amount while barely altering the applied load. In previous work, using numerical simulations, we investigated this behavior assuming that the magnetic moments carried by the embedded particles can freely reorient to minimize their magnetic interaction energy. Here, we extend the analysis to ferrogels where restoring torques by the surrounding matrix hinder rotations towards a magnetically favored configuration. For example, the particles can be chemically cross-linked into the polymer matrix and the magnetic moments can be fixed to the particle axes. We demonstrate that these systems still feature a superelastic regime. As before, the nonlinear stress-strain behavior can be reversibly tailored during operation by external magnetic fields. Yet, the different coupling of the magnetic moments causes different types of response to external stimuli. For instance, an external magnetic field applied parallel to the stretching axis hardly affects the superelastic regime but stiffens the system beyond it. Other smart materials featuring superelasticity, e.g. metallic shape-memory alloys, have already found widespread applications. Our soft polymer systems offer many additional advantages such as a typically higher deformability and enhanced biocompatibility combined with high tunability.

Structural control of elastic moduli in ferrogels and the importance of non-affine deformations.

One of the central appealing properties of magnetic gels and elastomers is that their elastic moduli can reversibly be adjusted from outside by applying magnetic fields. The impact of the internal magnetic particle distribution on this effect has been outlined and analyzed theoretically. In most cases, however, affine sample deformations are studied and often regular particle arrangements are considered. Here we challenge these two major simplifications by a systematic approach using a minimal dipole-spring model. Starting from different regular lattices, we take into account increasingly randomized structures, until we finally investigate an irregular texture taken from a real experimental sample. On the one hand, we find that the elastic tunability qualitatively depends on the structural properties, here in two spatial dimensions. On the other hand, we demonstrate that the assumption of affine deformations leads to increasingly erroneous results the more realistic the particle distribution becomes. Understanding the consequences of the assumptions made in the modeling process is important on our way to support an improved design of these fascinating materials.

Scaling of cluster growth for coagulating active particles.

Cluster growth in a coagulating system of active particles (such as microswimmers in a solvent) is studied by theory and simulation. In contrast to passive systems, the net velocity of a cluster can have various scalings dependent on the propulsion mechanism and alignment of individual particles. Additionally, the persistence length of the cluster trajectory typically increases with size. As a consequence, a growing cluster collects neighboring particles in a very efficient way and thus amplifies its growth further. This results in unusual large growth exponents for the scaling of the cluster size with time and, for certain conditions, even leads to "explosive" cluster growth where the cluster becomes macroscopic in a finite amount of time.

Tunable dynamic response of magnetic gels: impact of structural properties and magnetic fields.

Ferrogels and magnetic elastomers feature mechanical properties that can be reversibly tuned from outside through magnetic fields. Here we concentrate on the question of how their dynamic response can be adjusted. The influence of three factors on the dynamic behavior is demonstrated using appropriate minimal models: first, the orientational memory imprinted into one class of the materials during their synthesis; second, the structural arrangement of the magnetic particles in the materials; and third, the strength of an external magnetic field. To illustrate the latter point, structural data are extracted from a real experimental sample and analyzed. Understanding how internal structural properties and external influences impact the dominant dynamical properties helps to design materials that optimize the requested behavior.